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Journal Article

Polaritonic Chemistry: Collective Strong Coupling Implies Strong Local Modification of Chemical Properties

MPS-Authors
/persons/resource/persons251779

Sidler,  D.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
The Hamburg Center for Ultrafast Imaging;

/persons/resource/persons180973

Schäfer,  C.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
The Hamburg Center for Ultrafast Imaging;

/persons/resource/persons30964

Ruggenthaler,  M.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
The Hamburg Center for Ultrafast Imaging;

/persons/resource/persons22028

Rubio,  A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
The Hamburg Center for Ultrafast Imaging;
Center for Computational Quantum Physics, Flatiron Institute;

External Ressource
Fulltext (public)

acs.jpclett.0c03436.pdf
(Publisher version), 3MB

Supplementary Material (public)

jz0c03436_si_002.pdf
(Supplementary material), 8MB

Citation

Sidler, D., Schäfer, C., Ruggenthaler, M., & Rubio, A. (2021). Polaritonic Chemistry: Collective Strong Coupling Implies Strong Local Modification of Chemical Properties. The Journal of Physical Chemistry Letters, 12(1), 508-516. doi:10.1021/acs.jpclett.0c03436.


Cite as: http://hdl.handle.net/21.11116/0000-0007-5ABA-3
Abstract
A fundamental question in the field of polaritonic chemistry is whether collective coupling implies local modifications of chemical properties scaling with the ensemble size. Here we demonstrate from first-principles that an impurity present in a collectively coupled chemical ensemble features such locally scaling modifications. In particular, we find the formation of a novel dark state for a nitrogen dimer chain of variable size, whose local chemical properties are altered considerably at the impurity due to its embedding in the collectively coupled environment. Our simulations unify theoretical predictions from quantum optical models (e.g., collective dark states and bright polaritonic branches) with the single molecule quantum chemical perspective, which relies on the (quantized) redistribution of charges leading to a local hybridization of light and matter. Moreover, our findings suggest that recently developed ab initio methods for strong light-matter coupling are suitable to access these local polaritonic effects and provide a detailed understanding of photon-modified chemistry.